Numerical simulation results of a single-jet premixed combustion system at atmospheric pressure are compared against comprehensive particle image velocimetry (PIV) flow measurements and Raman scattering temperature measurements for natural gas and hydrogen fuels. The simulations were performed on hexahedral meshes with 1–5 × 106 elements. Reynolds-averaged Navier–Stokes (RANS) calculations were carried out with the k–ε realizable turbulence model. Combustion was modeled using the flamelet-generated manifold model (FGM) and detailed chemistry. Both the flame position and flame liftoff predicted by the FGM were in reasonable agreement with experiments for both fuels and showed little sensitivity to heat transfer or radiation modeling. The detailed chemistry calculation predicts the temperature gradients along the jet centerline accurately and compares very closely with the Raman scattering measurements. The much closer agreement of the jet axial velocity and temperature profiles with experimental values, coupled with the significantly protracted presence of intermediates in the detailed chemistry predictions, indicates that the impact of nonequilibrium intermediates on very lean natural gas flames is significant.